Design principles of practical industrial-scale layered oxide cathodes with air/water stability for sustainable sodium-ion batteries
Xin‐Bei Jia, Qianqian Peng, Yi‐Feng Liu, Dian-Cheng Chen, Jingqiang Wang, Jiayang Li, Yan‐Fang Zhu, Nan Xu, Lingyi Kong, Hanxiao Liu, Guangyu Zhang, Zhuang‐Chun Jian, Cheng Chen, Hanghang Dong, Liang Zhang, Yang Sun, Shuangqiang Chen, Xiaodong Guo, Shixue Dou, Yao Xiao
Abstract
Low-cost manganese-based oxides as promising cathodes for sodium-ion batteries still face significant challenges, including irreversible phase transition, air/water sensitivity, and low initial charge capacity. Herein, we precisely design a titanium-substituted Mn-based oxide cathode material with optimized local electronic structure distribution through a stepwise screening mechanism based on theoretical calculations, which enables suppression of irreversible phase transition and Jahn-Teller distortion by exerting spring effect and pinning effect. Notably, the optimized cathode fabricated using an aqueous binder exhibits stable electrochemical performance, retaining 96.16 % of its capacity after 500 cycles at 1 A g−1, along with reliable air/water stability under prolonged exposure, which is further confirmed by advanced characterization and theoretical calculations. In addition, Prussian blue analogs are proposed as a sodium supplement for full cell applications. The large-scale production and implementation of composite cathode materials have been successfully achieved and subsequently applied in practical pouch cells with non-presodiated hard carbon anodes. This work investigates an air/water-stable Mn-based layered oxide cathode for sodium-ion batteries, providing insights relevant to their future industrial development. Manganese-based oxides are promising cathodes for sodium-ion batteries. Here, authors design a titanium substituted oxide cathode with an optimized structure, achieving long cycle life, good air/water stability, and validation in pouch cells, supported by theory and experiments.